CN104134816A - Three-dimensional all-solid-state mini thin-film lithium battery with inverted pyramid array structure - Google Patents

Three-dimensional all-solid-state mini thin-film lithium battery with inverted pyramid array structure Download PDF

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Publication number
CN104134816A
CN104134816A CN201410380855.1A CN201410380855A CN104134816A CN 104134816 A CN104134816 A CN 104134816A CN 201410380855 A CN201410380855 A CN 201410380855A CN 104134816 A CN104134816 A CN 104134816A
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Prior art keywords
film
anode
solid
current collector
array structure
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郭航
林杰
郭建来
刘畅
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Xiamen University
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Xiamen University
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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/052—Li-accumulators
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/058—Construction or manufacture
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/10—Energy storage using batteries
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
    • Y02P70/50—Manufacturing or production processes characterised by the final manufactured product

Abstract

The invention discloses a three-dimensional all-solid-state mini thin-film lithium battery with an inverted pyramid array structure, and relates to lithium batteries. The three-dimensional all-solid-state mini thin-film lithium battery is provided with a substrate, an insulation film, a cathode current collector, a lower anode current collector, a cathode film, a solid electrolyte film, an anode film and an upper anode current collector, wherein the insulation film is arranged on the substrate; the cathode current collector and the lower anode current collector are arranged on the insulation film; the cathode film is arranged on the cathode current collector; the solid electrolyte film covers the cathode film; the anode film is arranged on the solid electrolyte film; the upper anode current collector is arranged on the anode film and the lower anode current collector. Based on the anisotropic etching of a silicon substrate, the inverted pyramid array structure is precisely manufactured and applied to the all-solid-state mini thin-film lithium battery, so that the capacity of active substances in unit standing area is improved and the contact between the thin films is tight. According to the unique design of a mask, the upper and lower circuits are guided to a same plane, so that the space utilization rate and the structure stability of the mini battery are effectively improved.

Description

A kind of three-dimensional full-solid-state minisize film lithium cell that adopts inverted pyramid array structure
Technical field
The present invention relates to lithium battery, especially relate to a kind of three-dimensional full-solid-state minisize film lithium cell that adopts inverted pyramid array structure.
Background technology
Now, along with developing rapidly of MEMS (micro electro mechanical system) (MEMS), external power supply cannot meet growing microminiaturization, integrated demand.Miniature thin-film lithium battery due to its size flexibly, the advantage such as safety and high-energy-density, in micro-energy, show one's talent.But existing all solid-state thin-film lithium battery major part is all confined to ([1] K.F.Chiu, C.C.Chen, K.M.Lin, H.C.Lin, C.C.Lo, W.H.Ho, C.S.Jiang, Vacuum, 84 (2010) 1296-1301 in two dimensional surface; [2] J.F.Whitacre, W.C.West, B.V.Ratnakumar, J Electrochem Soc, 150 (2003) A1676; [3] B.J.Neudecker, N.J.Dudney, J.B.Bates, J Electrochem Soc, 147 (2000) 517-523), space availability ratio is low, even existing three-dimension film lithium battery, conventionally complex structure, higher ([4] L.Baggetto of technological requirement, R.A.H.Niessen, F.Roozeboom, P.H.L.Notten, Adv Funct Mater, 18 (2008) 1057-1066; [5] L.Baggetto, H.C.M.Knoops, R.A.H.Niessen, W.M.M.Kessels, P.H.L.Notten, J MaterChem, 20 (2010) 3703), most of rectangle or column three-dimensional structure ([6] M.Kotobuki, Y.Suzuki adopting, H.Munakata, K.Kanamura, Y.Sato, K.Yamamoto, T.Yoshida, J Electrochem Soc, 157 (2010) A493; [7] D.Golodnitsky, V.Yufit, M.Nathan, I.Shechtman, T.Ripenbein, E.Strauss, S.Menkin, E.Peled, J Power Sources, 153 (2006) 281-287), be difficult for being combined with microelectronic technique, be often that single electrode maybe needs to add electrolyte ([8] K.Yoshima, H.Munakata, K.Kanamura, J Power Sources, 208 (2012) 404-408; [9] T.Ripenbein, D.Golodnitsky, M.Nathan, E.Peled, Electrochimica Acta, 56 (2010) 37-41), thereby inreal microminiaturized, the full battery of solidification, and seldom have researcher to consider the planar design of circuit, upper circuit lead to the basal surface of hull cell is encapsulated.
Summary of the invention
In order to overcome above-mentioned the deficiencies in the prior art, the invention provides a kind of three-dimensional full-solid-state minisize film lithium cell that adopts inverted pyramid array structure.
The present invention is provided with substrate, dielectric film, cathode current collector, lower floor's anode collector, cathodic coating, solid electrolyte film, anode film and upper strata anode collector;
Described dielectric film is located on substrate, cathode current collector and lower floor's anode collector are located on dielectric film, and cathodic coating is located on cathode current collector, and solid electrolyte film covers on cathodic coating, anode film is located on solid electrolyte film, and upper strata anode collector is located in anode film and lower floor's anode collector.
Three-dimensional structure is to utilize SiO 2work as masking layer, the silicon in <100> crystal orientation is done anisotropic etch and obtained with KOH solution.
Described substrate can adopt the silicon chip in <100> crystal orientation, and described dielectric film can adopt SiO 2film or Si 3n 4film, described cathode current collector, lower floor's anode collector and upper strata anode collector can adopt Pt, Au, Ni, Cu or Al, described cathode current collector, the preferred Pt of lower floor's anode collector, the preferred Cu of upper strata anode collector.
Described cathodic coating can adopt the oxidation film of lithium film or metal, preferably LiCoO 2film; Described solid electrolyte film is the LiPON film of LiPON film or modification, preferably LiPON film; Described anode film can be metal or metal oxide film, preferably SnO xfilm.
The area of described cathodic coating can be 0.1～1mm 2, thickness can be 0.1～2 μ m, preferably area 0.65mm × 0.8mm, thickness 0.6 μ m; The thickness of described solid electrolyte film can be 0.1～2 μ m, preferably 0.6 μ m; The thickness of described anode film can be 0.1～2 μ m, preferably 0.2 μ m.
Described cathodic coating carries out 300～1000 DEG C of annealing in process in oxygen or air, preferably 700 DEG C of annealing in process.
Described dielectric film can be by oxidizing process or chemical vapour deposition technique preparation; Described cathode current collector, lower floor's anode collector, cathodic coating, solid electrolyte film, anode film and upper strata anode collector all can be by magnetron sputtering method or pulsed laser deposition preparations.
The present invention utilizes the anisotropic etch of silicon substrate, accurately produce inverted pyramid array structure, and be applied in full-solid-state minisize film lithium cell, improve unit and based oneself upon the active material load capacity in area, and made the contact between each layer film tightr.Adopting unique mask plate design simultaneously, upper and lower circuit is caused to same plane, is the space availability ratio that improves micro cell, the effective means of structural stability.
Compared with prior art, the invention has the beneficial effects as follows:
1, silica-based and three-dimensional microstructures and microelectronic technique compatibility, easily realization and microdevice is integrated.
2, technique continuity is good, device integrity is good, has prepared rear protection metal pair minicell, especially solid electrolyte and has had good sealing and drainage.
3, designed three-dimensional structure and the identical two-dimensional structure contrast of basing oneself upon area, its contact area has improved 30%, and the chemical property of minicell can be significantly improved.
4, electric current is caused lower floor by upper strata collector, follow-uply realizes the circuit design in plane and need not carry out other lead-in wire.
Brief description of the drawings
Fig. 1 is the cross-sectional view of the embodiment of the present invention;
Fig. 2 is the vertical view of the embodiment of the present invention;
Fig. 3 is the vertical view of embodiment of the present invention inverted pyramid array;
Fig. 4 is the design drawing of embodiment of the present invention inverted pyramid structure.
Embodiment
Below in conjunction with accompanying drawing, the present invention will be further described.
As shown in Fig. 1～4, the embodiment of the present invention is provided with substrate 1, dielectric film 2, cathode current collector 3a, the anode collector 3b of lower floor, cathodic coating 4, solid electrolyte film 5, anode film 6 and upper strata anode collector 7.
Described dielectric film 2 is located on substrate 1, cathode current collector 3a and the anode collector 3b of lower floor are located on dielectric film 2, cathodic coating 4 is located on cathode current collector 3a, solid electrolyte film 5 covers on cathodic coating 4, anode film 6 is located on solid electrolyte film 5, and upper strata anode collector 7 is located on anode film 6 and the anode collector 3b of lower floor.
Three-dimensional structure is to utilize SiO 2work as masking layer, the silicon in <100> crystal orientation is done anisotropic etch and obtained with KOH solution.
Described substrate 1 can adopt the silicon chip in <100> crystal orientation, and described dielectric film 2 can adopt SiO 2film or Si 3n 4film, described cathode current collector 3a, the anode collector 3b of lower floor and upper strata anode collector 7 can adopt Pt, Au, Ni, Cu or Al, described cathode current collector 3a, the preferred Pt of the anode collector 3b of lower floor, the preferred Cu of upper strata anode collector 7.
Described cathodic coating 4 can adopt the oxidation film of lithium film or metal, preferably LiCoO 2film; Described solid electrolyte film 5 is the LiPON film of LiPON film or modification, preferably LiPON film; Described anode film 6 can be metal or metal oxide film, preferably SnO xfilm.
The area of described cathodic coating 4 can be 0.1～1mm 2, thickness can be 0.1～2 μ m, preferably area 0.65mm × 0.8mm, thickness 0.6 μ m; The thickness of described solid electrolyte film 5 can be 0.1～2 μ m, preferably 0.6 μ m; The thickness of described anode film 6 can be 0.1～2 μ m, preferably 0.2 μ m.
Described cathodic coating 4 carries out 300～1000 DEG C of annealing in process in oxygen or air, preferably 700 DEG C of annealing in process.
Described dielectric film 2 can be by oxidizing process or chemical vapour deposition technique preparation; Described cathode current collector 3a, the anode collector 3b of lower floor, cathodic coating 4, solid electrolyte film 5, anode film 6 and upper strata anode collector 7 all can be by magnetron sputtering method or pulsed laser deposition preparations.
First adopt <100> standard silicon chip, be all oxidized one deck SiO in upper and lower surface 2, then make the three-dimensional corrosion window of 500 μ m × 500 μ m by lithography.Then with SiO 2for masking layer, silicon is carried out to wet etching with KOH solution, obtain three-dimensional structure as shown in Figures 3 and 4, the structure eroding away and the angle of plane are α=54.7 °.Remove again original SiO 2, be again oxidized the dielectric isolation layer that one deck is new.Then on substrate, apply photoresist, form current collector window after photoetching, the Cr of first sputter layer is as sticky glutinous layer, the thicker Pt of sputter one deck is as cathode current collector and lower floor's anode collector, then in acetone, peels off unnecessary metal.Similarly, after gluing, make the anodal window of 500 μ m × 500 μ m by lithography, then the thick LiCoO of the about 600nm of sputter one deck 2as cathodic coating, then peel off unnecessary material with acetone.In order to reduce membrane stress and to realize crystallization, whole substrate is placed in oxygen atmosphere, with 700 DEG C of annealing 2h.After gluing, make the window of electrolyte and negative pole by lithography, the thick LiPON of the about 600nm of sputter one deck is as solid electrolyte film, the thicker SnO of the about 200nm of sputter one deck simultaneously xas anode film, then peel off unnecessary material with acetone.The Cu that finally sputter one deck is thicker is as upper strata anode collector film, and then gluing makes protective layer window by lithography, and corrodes and obtain last structure with strong acid solution.

Claims (10)

1. a three-dimensional full-solid-state minisize film lithium cell that adopts inverted pyramid array structure, is characterized in that being provided with substrate, dielectric film, cathode current collector, lower floor's anode collector, cathodic coating, solid electrolyte film, anode film and upper strata anode collector;
Described dielectric film is located on substrate, cathode current collector and lower floor's anode collector are located on dielectric film, and cathodic coating is located on cathode current collector, and solid electrolyte film covers on cathodic coating, anode film is located on solid electrolyte film, and upper strata anode collector is located in anode film and lower floor's anode collector.
2. a kind of three-dimensional full-solid-state minisize film lithium cell that adopts inverted pyramid array structure as claimed in claim 1, is characterized in that described substrate adopts the silicon chip in <100> crystal orientation.
3. a kind of three-dimensional full-solid-state minisize film lithium cell that adopts inverted pyramid array structure as claimed in claim 1, is characterized in that described dielectric film adopts SiO 2film or Si 3n 4film.
4. a kind of three-dimensional full-solid-state minisize film lithium cell that adopts inverted pyramid array structure as claimed in claim 1, it is characterized in that described cathode current collector, lower floor's anode collector and upper strata anode collector adopt Pt, Au, Ni, Cu or Al, described cathode current collector, the preferred Pt of lower floor's anode collector, the preferred Cu of upper strata anode collector.
5. a kind of three-dimensional full-solid-state minisize film lithium cell that adopts inverted pyramid array structure as claimed in claim 1, is characterized in that described cathodic coating adopts the oxidation film of lithium film or metal, preferably LiCoO 2film; The area of described cathodic coating can be 0.1～1mm 2, thickness can be 0.1～2 μ m, preferably area 0.65mm × 0.8mm, thickness 0.6 μ m.
6. a kind of three-dimensional full-solid-state minisize film lithium cell that adopts inverted pyramid array structure as claimed in claim 1, is characterized in that described solid electrolyte film is the LiPON film of LiPON film or modification, preferably LiPON film; The thickness of described solid electrolyte film can be 0.1～2 μ m, preferably 0.6 μ m.
7. a kind of three-dimensional full-solid-state minisize film lithium cell that adopts inverted pyramid array structure as claimed in claim 1, is characterized in that described anode film is metal or metal oxide film, preferably SnO xfilm; The thickness of described anode film can be 0.1～2 μ m, preferably 0.2 μ m.
8. a kind of three-dimensional full-solid-state minisize film lithium cell that adopts inverted pyramid array structure as claimed in claim 1, is characterized in that described cathodic coating carries out 300～1000 DEG C of annealing in process in oxygen or air, preferably 700 DEG C of annealing in process.
9. a kind of three-dimensional full-solid-state minisize film lithium cell that adopts inverted pyramid array structure as claimed in claim 1, is characterized in that described dielectric film is by oxidizing process or chemical vapour deposition technique preparation.
10. a kind of three-dimensional full-solid-state minisize film lithium cell that adopts inverted pyramid array structure as claimed in claim 1, is characterized in that described cathode current collector, lower floor's anode collector, cathodic coating, solid electrolyte film, anode film and upper strata anode collector are all by magnetron sputtering method or pulsed laser deposition preparation.
CN201410380855.1A 2014-08-05 2014-08-05 Three-dimensional all-solid-state mini thin-film lithium battery with inverted pyramid array structure Pending CN104134816A (en)

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CN106848390A (en) * 2016-12-05 2017-06-13 东莞市绿骏电动自行车科技有限公司 A kind of film lithium cell of 3D structures
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Cited By (13)

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Publication number Priority date Publication date Assignee Title
CN105449168A (en) * 2015-11-19 2016-03-30 中国航空工业集团公司北京航空材料研究院 Preparation method of metal matrix solid-state thin-film lithium battery cathode with interface modification layer
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WO2017180945A1 (en) * 2016-04-14 2017-10-19 Applied Materials, Inc. Energy storage device with encapsulation anchoring
CN106058305A (en) * 2016-08-12 2016-10-26 合肥国轩高科动力能源有限公司 Method for in-situ preparation of minisized all-solid-state thin-film lithium-ion battery by using PLD
CN106848390B (en) * 2016-12-05 2019-02-01 东莞市绿骏电动自行车科技有限公司 A kind of film lithium cell of 3D structure
CN106848390A (en) * 2016-12-05 2017-06-13 东莞市绿骏电动自行车科技有限公司 A kind of film lithium cell of 3D structures
CN108325876A (en) * 2017-12-19 2018-07-27 成都亦道科技合伙企业（有限合伙） Lithium battery material high-throughput screening method
CN109817972A (en) * 2019-01-24 2019-05-28 深圳市致远动力科技有限公司 All solid-state thin-film lithium battery with micro-nano structure
WO2021059045A1 (en) * 2019-09-23 2021-04-01 International Business Machines Corporation High capacity compact lithium thin film battery
CN114424377A (en) * 2019-09-23 2022-04-29 国际商业机器公司 High-capacity compact lithium thin film battery
GB2602607A (en) * 2019-09-23 2022-07-06 Ibm High capacity compact lithium thin film battery
GB2602607B (en) * 2019-09-23 2023-05-17 Ibm High capacity compact lithium thin film battery

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